Charged particle measuring device and measuring method thereof

ABSTRACT

A highly sensitive charged particle measuring device capable of measuring low-level alpha rays comprises in a measurement chamber  7  provided with a sealable door  15 , a test sample  2  and a semiconductor detector  1 , a radiation measuring circuit  30  including a preamplifier  30   c  connected to the semiconductor detector  1 , a linear amplifier  30   d , and a pulse height analyzer  30   e , a charged particle emission amount arithmetic unit  40  for performing the quantitative analysis of charged particles from its measurement, a display unit for displaying its analysis result, and further has an evacuation pipe line and a pure gas supply pipe line for performing supply and replacement of the pure gas in the measuring chamber  7.

BACKGROUND OF THE INVENTION

[0001] 1. Field of the Invention

[0002] The present invention relates to a charged particle measuringdevice and a measuring method for measuring charged particles such aslow-level alpha rays, and in particular to a charged particle measuringdevice and measuring method suitable for the quantitative analysis ofcharged particles such as low-level alpha rays in various materials.

[0003] 2. Description of the Related Art

[0004] Conventional art will be described in particular for themeasurement of alpha rays among various types of charged particles.

[0005] As conventional technology, there is a gas flow-proportionalcounter type low-level alpha ray measuring device mentioned in “asuper-low-level alpha ray measuring device”, Electronic Material, August1988, p. 91. This apparatus is a gas flow-proportional counter with adetection area of 1000 cm², and a detector where cathodes are arrangedabove and below a multiple wire type anodes disposed at the center. Atest sample is directly put into the detector, and is placed closely tothe lower side of a grid-like lower cathode. A counting gas is flown ata rate of about 200 ml per minute, the counting gas being a PR gas whichis a mixed gas of argon and methane, and several thousands volts of DCvoltage is applied to between the anodes and cathodes. When an alphaparticle enters into the detector, the gas is ionized, and a short pulsecurrent flows. Hence, the number of alpha particles is counted byconverting this current into a voltage pulse and counting them.

[0006] In order to take countermeasures against problems such as a softerror phenomenon where stored charges in a semiconductor memory arereversed by alpha particles, the problem being caused by semiconductormemories becoming finer, it is important to perform a nuclideidentification and low-level quantitative analysis of a disturbancealpha ray that a trace natural alpha emission element included invarious material emits.

[0007] Although it can easily measure a sample with a large area, theabove-described conventional gas flow-proportional counter typelow-level alpha ray measuring device needs to apply several thousandsvolts of DC voltage to between the anodes and cathodes of the detector,and needs to perform measurement while flowing PR gas as the countinggas. Hence, the apparatus becomes large in size.

[0008] In addition, in the performance of alpha ray analysis, there aremajor defects that energy resolution is inferior, that discriminatingmeasurement of an alpha ray nuclide is not possible, and that abackground discrete value cannot be made small, and hence, lower-levelalpha ray measurement cannot be performed.

SUMMARY OF THE INVENTION

[0009] A first object of the present invention is to provide a chargedparticle measuring device with high sensitivity that can efficientlymeasure charged particles such as a low-level alpha ray whose nuclide isidentified, and a measuring method thereof.

[0010] A second object of the present invention is to provide a chargedparticle measuring device that can realize the measurement of chargedparticles such as a lower-level alpha ray, and a measuring methodthereof.

[0011] A third object of the present invention is to provide a chargedparticle measuring device which can reduce the background discretevalue, and a measuring method thereof.

[0012] A fourth object of the present invention is to provide a chargedparticle measuring device which is not a large-scale apparatus, but canrealize the measurement of charged particles such as a lower-level alpharay, and a measuring method thereof.

[0013] To achieve the above-described objects, a charged particlemeasuring device according to the present invention is characterized incomprising a measuring chamber having a sealing door which can be openedand closed, the measuring chamber comprising: a semiconductor detector;a radiation measuring circuit including a sample tray on which ameasurement sample is placed so as to oppose to the semiconductordetector, a preamplifier, a linear amplifier, and a pulse heightanalyzer connected to the semiconductor detector; a charged particleemission amount arithmetic unit for performing the quantitative analysisof charged particles with an output signal from the radiation measuringcircuit; a display unit for displaying the analysis result of thecharged particle emission amount arithmetic unit; and including: anevacuation pipe line for discharging air to the measuring chamber; and apure gas supply pipe line for performing the supply and replacement of apure gas.

[0014] In addition, a charged particle measuring device according to thepresent invention is characterized in comprising a measuring chamber,the measuring chamber comprising: a semiconductor detector; ameasurement sample placed so as to oppose to the semiconductor detector;a radiation measuring circuit which includes a shield shutter that isarranged between the semiconductor detector and the sample and shieldscharged particles entering from the sample at the time of backgroundmeasurement, and is connected to the semiconductor detector to performspectrum analysis; a charged particle emission amount measuring devicewhich performs the quantitative analysis of charged particles with anoutput signal of the radiation measuring circuit; a display unit fordisplaying the analysis result of the charged particle emission amountmeasuring device, and including an evacuation apparatus and a gasreplacement apparatus, which are connected through an exhaust pipe whichcommunicates with the measuring chamber.

[0015] Furthermore, a charged particle measuring method according to thepresent invention is characterized in comprising the steps of: arranginga sample tray on which a test sample is placed so as to oppose to asemiconductor detector in a measuring chamber having a sealable doorwhich can be opened and closed; performing cycle purge for apredetermined number of times with a pure gas by an evacuation apparatusand a gas replacement apparatus which are connected through an exhaustpipe which communicates with the inside of the measuring chamber, andthereafter measuring a charged particle emission amount by a radiationmeasuring circuit which includes a preamplifier, a linear amplifier, anda pulse height analyzer that are connected to the semiconductordetector, and a charged particle emission amount arithmetic unit forperforming quantitative analysis of charged particle with an outputsignal from the radiation measuring circuit, and setting the chargedparticle emission amount as a background measurement; and calculating acharged particle emission amount value which is obtained by subtractingthe background measurement from a measurement of the charged particleemission amount obtained by measuring a charged particle emission amountafter placing the sample on the sample tray and performing cycle purgefor a predetermined number of times with a pure gas.

[0016] Moreover, a charged particle measuring method according to thepresent invention is characterized in comprising the steps of: arranginga measurement sample so as to oppose to a semiconductor detector in ameasuring chamber; shielding charged particles entering from themeasurement sample by a shield shutter between the semiconductordetector and the sample; performing cycle purge for a predeterminednumber of times with a pure gas by an evacuation apparatus and a gasreplacement apparatus which are connected through an exhaust pipecommunicating with the inside of the measuring chamber, and thereaftermeasuring a charged particle emission amount by a radiation measuringcircuit which is connected with the semiconductor detector and performsspectrum analysis, and a charged particle emission amount measuringdevice which performs the quantitative analysis of charged particleswith an output signal of the radiation measuring circuit, and settingthe charged particle emission amount as a background measurement; andcalculating a charged particle emission amount value which is obtainedby subtracting the background measurement from a measurement of thecharged particle emission amount obtained by measuring a chargedparticle emission amount entering from the sample, by opening the shieldshutter.

BRIEF DESCRIPTION OF THE DRAWINGS

[0017]FIG. 1 is a structural diagram of a low-level alpha ray measuringdevice according to one embodiment of the present invention;

[0018]FIG. 2 is a sectional view taken on line A-A in FIG. 1 and showsthe detail of an automatic open/close type shield shutter;

[0019]FIG. 3 is a schematic measurement flow chart at the time whenlow-level alpha ray measurement is fully automated;

[0020]FIG. 4 is a measurement flow chart of gas replacement anddecompression operation;

[0021]FIG. 5 is a measurement flow chart of background measurementoperation and sample measurement operation;

[0022]FIG. 6 is a graph showing the relation between the alpha rayenergy resolution, the total absorption peak value shift, and the degreeof vacuum;

[0023]FIG. 7 is a graph showing the time-dependent change of thebackground measurement;

[0024]FIG. 8 is a structural diagram of a radiation measuring circuitfor a semiconductor detector according to this embodiment;

[0025]FIG. 9 is a graph showing the trend data of alpha ray measurement;

[0026]FIG. 10 includes graphs showing a calibration method of thechannel of a pulse height analyzer and the alpha ray energy in a wideenergy range;

[0027]FIG. 11 is a perspective view showing a modified example in thecase where a measuring chamber portion of the super low-level alpha raymeasurement apparatus according to this embodiment is semi-automated;

[0028]FIG. 12 is a flow chart of super-low level alpha ray measurementthat uses a semi-automatic measuring chamber;

[0029]FIG. 13 is a structural diagram showing an example where two ormore semiconductor detectors according to this embodiment are arranged;and

[0030]FIG. 14 is a structural diagram of a radiation measuring circuitin a plural sheet array type semiconductor detector.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0031] Hereafter, taking an alpha ray as charged particles, anembodiment of the present invention will be described with reference toFIGS. 1 to 14. FIG. 1 is a structural diagram of a low-level alpha raymeasuring device according to this embodiment. In the upper area insidea measuring chamber 7 (also called a measurement housing 7), aflat-plate type semiconductor detector 1 which detects a low-level alpharay is fixedly provided on a sealable door 15 described later, and asignal line 20 of the semiconductor detector 1 is taken out from theupper part of the measuring chamber 7. A measurement sample 2 is set soas to oppose to the semiconductor detector 1 on a sample tray 4 on anelevating device 5 in the measuring chamber 7 by opening and closing thesealable door 15, and the distance between the sample 2 andsemiconductor detector 1 is adjusted by raising and lowering theelevating device 5. An O-ring groove is provided in a flange of themeasuring chamber 7, and contact surfaces of an O-ring 18, fit into thisO-ring groove, and the sealable door 15 are mirror-finished.

[0032] An automatic open/close type shield shutter 3 for shielding alpharays incident from the sample 2 at the time of background measurement isprovided between the semiconductor detector 1 and the sample 2. In orderto shield disturbance alpha rays incident from an inside wall of themeasuring chamber 7 etc., a shield wall 6 is provided so as to surroundthe circumference of the semiconductor detector 1 and the sample 2. Thisshield wall 6 is for shielding disturbance alpha rays incident fromfaces other than faces of the sample.

[0033]FIG. 2 is a detailed drawing of the automatic open/close typeshield shutter 3. The shield shutter 3 comprises a shield sheet 3 a anda shutter mechanism 3 b. Although an aluminum foil having a thickness inthe order of 10 μm can shield an alpha ray sufficiently, inconsideration of durability, for example, an aluminum sheet having athickness of about 100 μm is used as the shield sheet 3 a. As for themovable range of the shield shutter 3 that is shown by an arrow in FIG.2, a stroke is set so as to be able to fully close the sample 2 at thetime of background measurement and to be able to fully open the sample 2at the time of sample measurement. Moreover, it is possible to reducethe influence of disturbance radiations such as cosmic rays by usingstainless steel material and the like having good processability for theinside of the measuring chamber 7, and making the outside of themeasuring chamber 7 double structure (not shown) with a shieldingmaterial such as lead with a thickness of several centimeters. It ispossible to lower the minimum value that can be measured by adoptingsuch constitution.

[0034] An exhaust pipe 10 is provided in the lower area of the measuringchamber 7, and this exhaust pipe 10 branches into two exhaust pipes. Oneis connected to an evacuation apparatus 11, and another is connected toa gas replacement apparatus 12.

[0035] The evacuation apparatus 11 is for exhausting gases in themeasuring chamber 7 and measuring the alpha ray under decompression inorder to prevent attenuation of the alpha ray caused by the gases thatexist between the semiconductor detector 1 and the sample 2. Theevacuation apparatus 11 comprises an electromagnetic gate valve 11 a anda vacuum pump 11 b, and the vacuum pump 11 b is connected to the exhaustpipe 10 through the electromagnetic gate valve 11 a.

[0036] The gas replacement apparatus 12 is for replacing the environmentof the measuring chamber 7 by a pure gas, i.e., a gas that does notinclude a radioactive gas, and comprises an electromagnetic gate valve12 a, a pressure regulator 12 b, and a chemical cylinder 12 c forreplacement. The chemical cylinder 12 c for replacement is connected tothe exhaust pipe 10 through the electromagnetic gate valve 12 a andpressure regulator 12 b. Besides nitrogen gas, any gas so long as it isa pure gas that does not include a radioactive gas, can be used as thegas.

[0037] Since radon (abbreviation: Rn) which is a decay product ofuranium and thoron (abbreviation: Tn) that is a decay product of thoriumare included in air, alpha rays emitted from the radon and thoron becomestrong disturbance radiations. By the gas replacement apparatus 12making replacement gas flow into the measuring chamber 7, a small amountof air that remains in the measuring chamber 7 can be discharged by theevacuation apparatus 11, and the radon and thoron can be discharged fromthe measuring chamber 7 by replacing air with a pure gas such as anitrogen gas.

[0038] Thus, by activating a vacuum pump and evacuating the air inside ameasurement housing to replace it with pure gas, it is possible toremove the disturbance radiations in the air.

[0039] A shock absorber 8 for intercepting vibration is provided betweenthe measuring chamber 7 and a frame 16 to prevent microphonic noise thatthe semiconductor detector 1 receives by vibration. Moreover, it isdesirable that the exhaust pipe 10 is a tube such as a flexible tubewith little propagation of vibration, and owing to this, it is possibleto prevent vibration such as an earthquake from transmitting through theexhaust pipe 10, causing signal noise. A vibration monitor 14 thatmonitors vibration in order to differentiate a usual signal from noisecaused by vibration is disposed at a location where the vibration of themeasuring chamber 7 can be measured, for example, in the measuringchamber or the frame 16. Even if vibration is prevented by the shockabsorber 8 or the exhaust pipe 10 formed of a flexible tube, there is apossibility that the generation of noise cannot be prevented when strongvibration arises. Hence, when a signal detected by the vibration monitor14 exceeds a threshold, the measurement data in a time zone when thesignal exceeds the threshold is excluded.

[0040] In this manner, since the transmission to the measurement housingfrom a frame is blocked by the shock absorber, it is possible to preventmicrophonic noise by vibration that a semiconductor detector receives.In addition, since the processing of automatically removing measurementdata in the time zone when vibration monitored by the vibration monitorexceeds a threshold is performed, it is possible to acquire data whileremoving noise caused by strong vibration.

[0041] Moreover, an automatic controller 13 is installed in the frame16, and this controller 13 automatically controls the electromagneticgate valves 11 a and 12 a, vacuum pump 11 b, vacuum level monitor 9, andshield shutter 3.

[0042] The signal detected by the semiconductor detector 1 is inputtedinto a radiation measuring circuit 30 through a signal line 20, and isgiven spectrum analysis by the radiation measuring circuit 30, and thengiven data processing by an alpha ray emission amount arithmetic unit40. The processing result is displayed by a display unit 50.

[0043] The outline of a measurement flow in the case where low-levelalpha ray measurement is fully automated will be described withreference to FIG. 3. At step 100, the sample 2 to be measured is set inthe measuring chamber 7. At step 101, air in the measuring chamber 7 isreplaced by a pure gas in order to exhaust disturbance nuclides includedin the air in the measuring chamber 7. At step 102, the inside of themeasuring chamber 7 is decompressed in order to suppress the decay ofalpha rays with gases, the shield shutter 3 in a chamber 7 is closed atstep 103, and background measurement is performed at step 104. After thecompletion of the background measurement, at step 105, a lowermeasurement limit is calculated and the result is displayed. At step106, the shield shutter 3 in the measuring chamber 7 is opened, at step107, the alpha ray measurement of the sample is performed, and a netalpha ray emission amount is calculated by subtracting the backgroundmeasurement from the alpha ray measurement, and its result is displayedat step 108.

[0044] Next, the detail of the gas replacement at step 101, and thedecompressing operation at step 102 of FIG. 3 will be described withreference to FIG. 4. At step 100, the measuring chamber 7 is opened andthe measurement sample 2 is set on the sample tray 4. The sealable door15 of the measuring chamber 7 is airtightly sealed, and the vacuum pump11 b is activated at step 109. The electromagnetic gate valve 11 a isopened at step 110 to evacuate air in the measuring chamber 7. At step111, the degree of vacuum is monitored by the vacuum level monitor 9,and if a set degree of vacuum is reached, the electromagnetic gate valve11 a is shut at step 112. Then, the vacuum pump 11 b is stopped at step113.

[0045] The electromagnetic gate valve 12 a is opened at step 114. Thesource pressure of the chemical cylinder 12 c is decompressed by thepressure regulator 12 b for performing preset so that the exit pressure(or secondary pressure) of the pressure regulator 12 b may become nearly80 to 90 kPa that is lower than atmospheric pressure. A replacement gasflows into the measuring chamber 7, and at step 115, before themeasuring chamber 7 reaches atmospheric pressure, the electromagneticgate valve 12 a is closed to stop the inflow of the replacement gas(step 116). The reason why the electromagnetic gate valve 12 a is closedto stop the inflow of the replacement gas before reaching atmosphericpressure is because the emission of the replacement gas may arise if thepressure of the replacement gas reaches the atmospheric pressure, andthere arises a possibility that radon and thoron may invade if air mixesin.

[0046] At step 117, it is determined whether the number of times of puregas replacement operation is equal to the set number of times, and if itis fewer than the set number of times, the vacuum pump 11 b in a vacuumsystem is operated again, and operation at steps 109 to 116 areexecuted. If the set number of times is reached, the vacuum pump 11 b isactivated at step 118. The electromagnetic gate valve 11 a is opened atstep 119 to evacuate air in the measuring chamber 7. At step 120, thedegree of vacuum is monitored by the vacuum level monitor 9, and if aset degree of vacuum is reached, the electromagnetic gate valve 11 a isshut at step 121. Then, the vacuum pump 11 b is stopped at step 122.This replacement operation is repeated for an appropriate number oftimes depending on necessity, for example, three to four times. Inaddition, if the pure gas can replace the air by one operation, thenumber of times can be set to one. After the environment of themeasuring chamber 7 is replaced by the pure gas and reaches the setdegree of vacuum, the process moves to background measurement operationat step 104, and sample measurement operation at step 107 of FIG. 3.

[0047] The detail of background measurement operation and samplemeasurement operation will be described with reference to FIG. 5. Afterthe environment of the measuring chamber 7 is replaced by the pure gasand reaches the set degree of vacuum, the shield shutter 3 arrangedbelow the semiconductor detector 1 is closed at step 103, and backgroundmeasurement operation is begun while shielding the alpha rays from thesample 2.

[0048] Although described in detail by reference to FIG. 6, the degreeof vacuum is monitored by the vacuum level monitor 9 at step 123 sincethe deterioration of energy resolution and the shift of a totalabsorption peak value arise if the degree of vacuum drops. Althoughdescribed in detail with reference to FIG. 7, since a counting rate ishigh just after measurement starts experientially, until time in theorder of 10 hours passes, a counting rate is sequentially calculated atstep 124 and data after the drop of the counting rate to an averagelevel is adopted.

[0049] In this manner, since a degree of vacuum is monitored by a vacuumlevel monitor and measurement data during the time when the degree ofvacuum exceeds a variance limit level is automatically removed, it ispossible to enhance alpha ray energy resolution and to acquire the datawith a small shift amount of total absorption peak values (energy) ofalpha rays.

[0050] Background measurement time is set to the time satisfying thelower alpha ray measurement limit being the target. Actually, a loweralpha ray measurement limit D (C/cm²·h) is calculated from formula 1.

[0051] [Formula 1]

D=3·(2·nb/tb)^(½)/(τ·Ad)   (1)

[0052] Here, nb denotes a background counting rate (cph), tb is abackground measuring time (h), τ is a detection efficiency, and Ad is anarea of a detecting element (cm²).

[0053] When it is determined at step 125 that the background measuringtime reaches the set time, measurement is stopped at step 126, and alower measurement limit is calculated and displayed by the alpha rayemission amount arithmetic unit 40 at step 105. When the backgroundmeasurement is completed, the shield shutter 3 arranged below thesemiconductor detector 1 is fully opened at step 106, and the processmoves on to sample measurement operation to measure alpha rays from thesample 2.

[0054] The degree of vacuum is monitored by the vacuum level monitor 9at step 127 since the deterioration of energy resolution and the shiftof a total absorption peak value occur if the degree of vacuum falls.The time determined by an alpha ray counting rate from the sample 2 isset as the measuring time of the sample 2 at step 128. Generally, if themeasured value of the sample is practically equal to that of thebackground, the measuring time is set equally to the backgroundmeasuring time. When it is determined at step 129 that the set time isreached, the measurement is stopped at step 130, an alpha ray emissionamount is calculated by the alpha ray emission amount arithmetic unit 40at step 108, and the net alpha ray emission amount obtained bysubtracting the background value is calculated. The net alpha rayemission amount Cα (C/cm²·h) is defined as a value calculated fromformula 2.

[0055] [Formula 2]

Cα=(nα−nb)/(τ·As)   (2)

[0056] Here, nα denotes an alpha ray counting rate (cph) of the sample,and nb is a background counting rate (cph), τ is a detection efficiency,and As is a sample area (cm²).

[0057] The degree of vacuum set at the above-described steps 111, 123,and 127 is set at about 1 kPa that belongs to a low vacuum region, i.e.,10 Torr. This is because, as shows in the first vertical axis of FIG. 6,the higher the degree of vacuum becomes, the better the alpha ray energyresolution becomes. Here, a smaller value represents a higher grade ofvacuum. On the other hand, since there is a certain electrical noisecomponent in a measurement system, for example, there is about 80% (0.08MeV) of electrical noise component in an example shown in FIG. 6, theeffect of resolution enhancement being low even if the level of vacuumis increased further. For this reason, in the example shown in FIG. 6,the pressure of about 1 kPa that belongs to a low vacuum region issuitable. In addition, as shown in the vertical secondary axis in FIG.6, since the shift amount of a total absorption peak value (energyshift) of an alpha ray becomes large as the degree of vacuum becomes low(a larger value means a lower grade of vacuum), it becomes important tomaintain the degree of vacuum at a set value also in prolongedmeasurement. Since the contact surface of the sealable door 15 with theO-ring 18 is mirror-finished, leak can be suppressed to a small volumeeven if a long time passes after evacuation stop. In addition, when theleak amount increases and a measurement of the vacuum level monitor 9exceeds a variance limit level, for example, 9 kPa, exclusion processingof the measurement data during the time after exceeding the variancelimit level is performed. If the measuring time runs short as a resultof exclusion processing, data accumulation is performed again afterperforming evacuation and returning to a set degree of vacuum. This dataprocessing is performed by, for example, the alpha ray emission amountarithmetic unit 40. Owing to the adoption of this method, thereliability of data is sharply securable.

[0058] The time-dependent change of the counting rate at the start ofthe measurement while setting the range of measurement energy to 5.5 to10 MeV is shown in FIG. 7. As seen from the result shown in FIG. 7, thecounting rate is high at the beginning of a measurement and when about25 hours passes, the counting rate drops to an average level, i.e., anaverage counting rate level of the background. When performing samplemeasurement immediately after performing gas replacement, the sametime-dependent change is shown. This can be considered to be theinfluence of alpha rays emitted by decay products of radon and thoronthat remain slightly in the measuring chamber 7. From this result, thesequence adopting the measurement data after time in the order of tenhours had passed when the counting rate becomes an average counting ratelevel, and automatically starting measurement after preset time elapsesafter the gas replacement becomes effective.

[0059] According to this embodiment, it is possible to realize 10⁻³(C/cm²·h) order of low-level alpha ray measurement that has not beenrealized up to now. Moreover, a 0.001 to 0.0001 (C/cm²·h) level or loweralpha ray measurement can be realized, and such a low-level alpha raymeasurement is called super low-level alpha ray measurement forconvenience.

[0060] Next, the configuration of the radiation measuring circuit 30connected to the signal line 20 of the semiconductor detector 1 will bedescribed with reference to FIG. 8.

[0061] In the subsequent stage of the signal line 20 of thesemiconductor detector 1 to which a bias voltage is applied by a biaspower supply 30 a, a coupling capacitor 30 b for reliable chargecollection, a preamplifier 30 c, and a linear amplifiers 30 d for pulseshaping matching for pulse height analysis are provided, and pulseheight is measured by a pulse height analyzer 30 e that is subsequent tothe linear amplifier 30 d. Alpha rays in an object energy range from theresult of the pulse height analysis is identified, the quantitativeanalysis of the alpha ray emission amount is performed by the alpha rayemission amount arithmetic unit 40, and its result is displayed on thedisplay unit 50. The alpha ray emission amount arithmetic unit 40monitors vibration with the vibration monitor 14, and also excludesnoise signal generated by an earthquake etc.

[0062]FIG. 9 shows the trend data of alpha ray measurement taking timeas the horizontal axis and taking the counting rate of alpha rays as thevertical axis. Since a measuring point A shown in FIG. 9 is generated atthe same time as when a signal of the vibration monitor 14 becomes high,which is the noise caused by strong vibration such as an earthquake, thedata at the measuring point A is excluded from measurement data. Inaddition, it is determined that a measuring point B is not caused byvibration but caused by electric waves etc., since the signal of thevibration monitor 14 is not high, and the data at the measuring point Bis excluded from the measurement data. The exclusion level of a noisesignal is determined by referring to a value of a statistical error σ ofcounting rate values. That is, processing sequence is that statisticalvariation is monitored to the average alpha ray counting rate per unittime, and if the statistical variation exceeds a set statisticalvariation reference value (this is also called a variance limit level),the measurement data within the unit time is automatically removed. Thisdata processing is performed by, for example, the alpha ray emissionamount arithmetic unit 40. Owing to the adoption of this method, it ispossible to realize reliable prolonged measurement.

[0063] Next, a method of calibrating the relation between the channel(this is also called a peak value) of a pulse height analyzer and thealpha ray energy in a large energy range will be described withreference to FIG. 10. Among decay products of uranium and thorium, thelargest alpha ray energy is 8.78 MeV of Po-212. However, common standardalpha ray sources are 5.49 MeV of Am-241, and 4.20 MeV and 4.78 MeV ofU-238, and usually, it is not possible to get these standard high-energyalpha ray sources. Therefore, by collecting the natural radon and thoronwhich are included in air and measuring Po-212 (8.78 MeV), Po-214 (7.69MeV), and Po-218 (6.00 MeV) of alpha rays which these decay productsemit, calibration in the large energy range is performed.

[0064] The radon and thoron are collected for a period of time in theorder of ten minutes in a basement of a building etc. by using anexhaust pump (this is also called a dust sampler) and a collectionfilter (this is also called a filter paper). The filter collecting theradon and thoron is set in the super low-level alpha ray measurementapparatus according to this embodiment. When the radon and thoron aremeasured, the gas replacement does not need to be performed and energycalibration is performed from the time course of alpha ray spectrum ofdecay products of the radon and thoron that are collected.

[0065] That is, at step 1 in FIG. 10, the collection filter collectingthe radon and thoron is set in the super low-level alpha ray measurementapparatus according to this embodiment. In the spectrum in one-hourmeasurement after two hours have passed from the collection in FIG. 10,Po-214 (7.69 MeV, half-life: 164 μa) that is a decay product of radon(Rn), is detected notably (step 2). In addition, Po-218 (6.00 MeV,half-life: 3.1 minutes) and Po-212 (8.78 MeV and half-life: 0.3 μs) thatis a decay product of thoron (Tn) are detected notably in the spectrumin 17-hour measurement after six hours have passed from the collectionin FIG. 10 (step 3). The relation between the alpha ray energy and thechannel of the pulse height analyzer is obtained from the totalabsorption peak value of these three nuclides and the alpha ray spectrumobtained from Am-241 that is a standard source by using a linearapproximation formula (step 4), and energy calibration is performed. Itbecomes possible to identify a nuclide of an alpha ray in a large energyrange from this energy calibration result. In addition, it becomespossible to determine a quantitative region of a nuclide to be measured,and to perform the quantitative analysis of the identified alpha ray.

[0066]FIG. 11 shows a modified example where a measuring chamber portionof the super low-level alpha ray measurement apparatus according to thisembodiment is semi-automated. The flat plate-type semiconductor detector1 that detects a super low-level alpha ray is provided in the upper partof the measuring chamber 7. The signal line 20 of the semiconductordetector 1 is taken out from the upper part of the measuring chamber 7.The sample 2 to be measured is placed on the sample tray 4 inserted intoa tray carrier 17 so that the sample 2 is opposed to the semiconductordetector 1 within the measuring chamber 7. The tray carrier 17 hasseveral steps so that the tray carrier 17 can correspond to thethickness of the test sample 2 and adjust the distance from thesemiconductor detector 1. This sample tray 4 serves also as a shieldwall for shielding the disturbance alpha rays emitted from the lowerinner wall of the measuring chamber 7. In addition, the tray carrier 17is integrated with a plate-like member in the lower rear side and servesalso as a shield wall for shielding the disturbance alpha rays emittedfrom the lower inner wall of the measuring chamber 7.

[0067] The exhaust pipe 10 for discharging gases in the measuringchamber 7 and performing measurement under decompression is provided onthe side wall of the measuring chamber 7, and is connected to theevacuation apparatus 11 and the gas replacement apparatus 12. Inaddition, the vacuum level monitor 9 for measuring the degree of vacuumin the measuring chamber 7 is provided. Since contact surfaces of theO-ring 18 and the sealable door 15 are mirror-finished, the amount ofleak can be suppressed to a small volume even if a long time passesafter evacuation stops.

[0068] Next, a semi-automatic measurement flow of a super-low levelalpha ray will be described with reference to FIG. 12. Measurement isperformed by two flows, a background measurement and a samplemeasurement.

[0069] First, a background measurement flow will be described. Themeasuring chamber 7 is opened and the sample tray 4 is set withoutplacing the sample 2. Then, the gas replacement and decompressionoperation are performed. These gas replacement and decompressionoperations are performed similar to the measurement flow of the fullyautomatic operation described in FIG. 4. When the gas replacement iscompleted and the vacuum level reaches a set value, the process advancesto the background measurement. Background measurement time is set so asto satisfy the lower alpha ray measurement limit being the target. Abackground counting rate and a lower measurement limit are calculated bythe alpha ray emission amount arithmetic unit 40 and displayed.

[0070] Next, in the sample measurement flow, the measuring chamber 7 isopened and the sample 2 is set on the sample tray 4. Then, the gasreplacement and decompression operation are performed. These gasreplacement and decompression operations are performed similar to themeasurement flow of the fully automatic operation described in FIG. 4.When the gas replacement is completed and the vacuum level reaches a setvalue, the process advances to the sample measurement. The measuringtime of the sample 2 is determined by an alpha ray counting rate fromthe test sample 2, and time is set. When the set time is reached, themeasurement is stopped, an alpha ray emission amount is obtained by thealpha ray emission amount arithmetic unit 40, and the net alpha rayemission amount obtained by subtracting the background value iscalculated and displayed.

[0071] Since it is necessary to manually set the sample in this method,measurement setup takes time, but since the shield shutter 3 is notnecessary, the configuration of the apparatus becomes simple, and hence,it is possible to realize a remarkably low cost apparatus.

[0072]FIG. 13 shows a modified example where two or more semiconductordetectors 1 of the super low-level alpha ray measurement apparatusaccording to this embodiment are arranged. The performance (this is alsocalled a lower measurement limit) of this measuring device is improvedas the detection area Ad becomes large as seen from formula 1, andhence, it is desirable to enlarge the detection area Ad as much aspossible. However, the size of the semiconductor detector 1 is limitedby the size of a crystal (this is also called wafer size). Therefore,the semiconductor detector in this embodiment secures the largerdetection area Ad by the configuration shown in FIG. 13. Namely, thesemiconductor detector 1 comprises a silicon device 1 a and itssubstrate 1 b, an electrode line wire 1 c, and fixing screws 1 d on thesubstrate, and in the example shown in FIG. 13, four pairs of silicondevices and their substrates 1 b are connected by the fixing screws 1 din the substrates and are electrically connected by the electrode linewires 1 c. It is possible to enhance the detection efficiency of thesemiconductor detectors 1 by approximating them as much as possible. Iffour sheets are arranged as shown in FIG. 13, measuring time iseffectively shortened to about one-fourth, and further super-low levelmeasurement can be realized. It becomes possible to enhance the lowermeasurement limit by enlarging the detection area, for example,increasing the number of sheets to eight sheets, or sixteen sheetsaccording to this method.

[0073] The configuration of a radiation measuring circuit of this pluralsheet array type semiconductor detector will be described with referenceto FIG. 14.

[0074] In the subsequent stage of the signal line 20 of thesemiconductor detector 1 to which a bias voltage is applied by a biaspower supply 30 a, a coupling capacitor 30 b for reliable chargecollection, a preamplifier 30 c, and a linear amplifiers 30 d for pulseshaping matching for pulse height analysis are provided. These areprovided to four semiconductor detectors 1, respectively, and signals ofrespective linear amplifiers are added by an adding amplifier 31 to bemeasured by a pulse height analyzer 30 e subsequent to the addingamplifier 31. Alpha rays in an energy range, which is an object range,from the result of the pulse height analysis is identified, thequantitative analysis of the alpha ray emission amount is performed bythe alpha ray emission amount arithmetic unit 40, and its result isdisplayed on the display unit 50.

[0075] Although the above explanation is described for the measurementof an alpha ray, the same measurement is possible also for chargedparticles such as beta rays.

[0076] As described above, according to this embodiment, it is possibleto provide a charged particle measuring device with high sensitivitythat can efficiently measure a super-low level of charged particle,which has been impossible up to now, while performing the nuclideidentification of the super-low level of charged particle.

[0077] According to this invention, it is possible to provide a chargedparticle measuring device with high performance that can efficientlymeasure a super-low level of charged particle.

What is claimed is:
 1. A charged particle measuring device comprising ameasuring chamber having a sealable door which can be opened and closed,the measuring chamber comprising: a semiconductor detector; a radiationmeasuring circuit including a sample tray on which a sample is placed soas to oppose to the semiconductor detector, a preamplifier, a linearamplifier, and a pulse height analyzer connected to the semiconductordetector; a charged particle emission amount arithmetic unit forperforming quantitative analysis of charged particles with an outputsignal from the radiation measuring circuit; a display unit fordisplaying analysis result of the charged particle emission amountarithmetic unit; an evacuation pipe line for exhausting air to themeasuring chamber; and a pure gas supply pipe line for supplying thepure gas for replacement.
 2. A charged particle measuring devicecomprising a measuring chamber, the measuring chamber comprising: asemiconductor detector; a sample placed so as to oppose to thesemiconductor detector; a radiation measuring circuit which includes ashield shutter that is arranged between the semiconductor detector andthe sample and shields charged particles incident from the sample duringbackground measurement, and is connected to the semiconductor detectorto perform a spectrum analysis; a charged particle emission amountmeasuring device which performs quantitative analysis of chargedparticles with an output signal of the radiation measuring circuit; adisplay unit for displaying analysis result of the charged particleemission amount measuring device; and an evacuation apparatus and a gasreplacement apparatus, which are connected through an exhaust pipecommunicating with the inside of the measuring chamber.
 3. The chargedparticle measuring device according to claim 1, wherein a vacuum levelmonitor is provided in the measuring chamber or an evacuation pipe line,and which starts remeasurement, after automatically removing measurementdata during the time when the degree of vacuum detected by the vacuumlevel monitor exceeds a variance limit level, and after performingevacuation of the inside of the measuring chamber and then performingsupply and replacement of a pure gas.
 4. The charged particle measuringdevice according to claim 2, wherein a vacuum level monitor is providedin the measuring chamber or an evacuation pipe line, and which startsremeasurement, after automatically removing measurement data during thetime when the degree of vacuum detected by the vacuum level monitorexceeds a variance limit level, and after performing evacuation of theinside of the measuring chamber and then performing supply andreplacement of a pure gas.
 5. The charged particle measuring deviceaccording to claim 1, wherein the charged particle measuring deviceincludes a vibration monitor for monitoring vibration of the measuringchamber, and automatically removes measurement data during the time whenthe degree of vacuum detected by the vacuum level monitor exceeds avariance limit level.
 6. The charged particle measuring device accordingto claim 2, wherein the charged particle measuring device includes avibration monitor for monitoring vibration of the measuring chamber, andautomatically removes measurement data during the time when the degreeof vacuum detected by the vacuum level monitor exceeds a variance limitlevel.
 7. The charged particle measuring device according to claim 1,wherein the charged particle emission amount arithmetic unit performsstatistical variation monitoring to an average charged particle countingrate per unit time, and further includes a processing sequence ofautomatically removing measurement data within the unit time when theaverage charged particle counting rate exceeds a statistical variationreference value that is set.
 8. The charged particle measuring deviceaccording to claim 2, wherein the charged particle emission amountarithmetic unit performs statistical variation monitoring to an averagecharged particle counting rate per unit time, and further includes aprocessing sequence of automatically removing measurement data withinthe unit time when the average charged particle counting rate exceeds astatistical variation reference value that is set.
 9. The chargedparticle measuring device according to claim 1, wherein a shield wallshielding disturbance charged particles incident from surfaces otherthan those of the sample is provided around a semiconductor detector ina measurement container, and an outer wall of the measuring chamber isfurther surrounded with a shielding material such as lead.
 10. Thecharged particle measuring device according to claim 2, wherein a shieldwall shielding disturbance charged particles incident from surfacesother than those of the sample is provided around a semiconductordetector in a measurement container, and an outer wall of the measuringchamber is further surrounded with a shielding material such as lead.11. The charged particle measuring device according to claim 1, whereinthe semiconductor detector is formed by connecting a plurality ofsilicon devices and substrates of the silicon devices with fixingscrews, and wiring them with electrode line wires, and a preamplifierand a linear amplifier are connected to each silicon deviceindividually, and an adder adding output signals of the respectivelinear amplifiers, a pulse height analyzer connected to the adder, and acharged particle emission amount arithmetic unit are provided.
 12. Thecharged particle measuring device according to claim 2, wherein thesemiconductor detector is formed by connecting a plurality of silicondevices and substrates of the silicon devices with fixing screws, andwiring them with electrode line wires, and a preamplifier and a linearamplifier are connected to each silicon device individually, and anadder adding output signals of the respective linear amplifiers, a pulseheight analyzer connected to the adder, and a charged particle emissionamount arithmetic unit are provided.
 13. A charged particle measuringmethod comprising the steps of: arranging a sample tray for placing asample so as to oppose to a semiconductor detector in a measuringchamber having a sealable door which can be opened and closed;performing several times of cycle purge with a pure gas by an evacuationapparatus and a gas replacement apparatus which are connected through anexhaust pipe which communicates with the inside of the measuringchamber; measuring a charged particle emission amount to set as abackground measurement using a radiation measuring circuit whichincludes a preamplifier, a linear amplifier, and a pulse height analyzerthat are connected to the semiconductor detector, and a charged particleemission amount arithmetic unit for performing quantitative analysis ofcharged particle with an output signal from the radiation measuringcircuit; and calculating a charged particle emission amount value whichis obtained by subtracting the background measurement from the chargedparticle emission amount measurement obtained by measuring a chargedparticle emission amount after placing the sample on the sample tray andperforming several times of cycle purge with a pure gas.
 14. A chargedparticle measuring method comprising the steps of: arranging a sample soas to oppose to a semiconductor detector in a measuring chamber;shielding charged particles incident from the sample by a shield shutterbetween the semiconductor detector and the sample, performing severaltimes of cycle purge with a pure gas by an evacuation apparatus and agas replacement apparatus which are connected through an exhaust pipewhich communicates with the inside of the measuring chamber; measuring acharged particle emission amount and setting the same as backgroundmeasurement value using a radiation measuring circuit which is connectedwith the semiconductor detector and performs spectrum analysis, and acharged particle emission amount measuring device which performsquantitative analysis of charged particles with an output signal of theradiation measuring circuit; and calculating a charged particle emissionamount value which is obtained by subtracting the background measurementfrom the charged particle emission amount measurement obtained bymeasuring a charged particle emission amount, incident from the testsample, by opening the shield shutter.
 15. The charged particlemeasuring method according to claim 13, including a sequence wheremeasurement data acquisition of the charged particle emission amount isstarted from a point of time when set time elapses after completing thecycle purge with a pure gas.
 16. The charged particle measuring methodaccording to claim 14, including a sequence where measurement dataacquisition of the charged particle emission amount is started from apoint of time when set time elapses after completing the cycle purgewith a pure gas.
 17. The charged particle measuring method according toclaim 13, characterized in that the charged particles form an alpha ray,and energy of the alpha ray to be measured is calibrated withmeasurement data of the alpha ray that a decay product emits that ismeasured using natural radon and thoron being collected.
 18. The chargedparticle measuring method according to claim 14, characterized in thatthe charged particles form an alpha ray, and energy of the alpha ray tobe measured is calibrated with measurement data of the alpha ray that adecay product emits that is measured using natural radon and thoronbeing collected.
 19. The charged particle measuring device according toclaim 1, wherein the charged particles form an alpha ray.
 20. Thecharged particle measuring method according to claim 13, wherein thecharged particles form an alpha ray.